Scholarlink

<p>Criegee intermediates are highly reactive species that play a pivotal role in the chemistry of the atmosphere, substantially impacting global climate and air quality. They are formed through the reaction of ozone with alkenes and considerably influence the formation of hydroxyl radicals and aerosols through their unimolecular decomposition and their reaction with key atmospheric components, respectively. However, their interaction with water vapour, a major atmospheric component, remains inadequately characterized. Here, using both time-dependent laser-induced fluorescence experiments and full-dimensional dynamics calculations, we investigate the reaction of <i>syn</i>-CH<sub>3</sub>CHOO, a prevalent Criegee intermediate, with water vapour. Our results reveal a much higher reaction rate than previously estimated, challenging the conventional notion that unimolecular decomposition dominates <i>syn</i>-CH<sub>3</sub>CHOO removal. Notably, we uncover a complex mechanism involving a roaming process that enhances reactivity. Our findings necessitate a revised assessment of reactions involving <i>syn</i>-mono- and di-substituted Criegee intermediates with water, which are crucial for accurately estimating the OH budget derived from these intermediates.</p><p></p>

错误：搜索内容不能为空，请输入英文关键词
错误：关键词超出字数限制，请精简
高级检索

Reactivity of syn-CH3CHOO with H2O enhanced through a roaming mechanism in the entrance channel

  • 期刊论文

  • 发表日期：

    2025年4月16日

查看全文
  • Yiqiang Liu,
  • Lijie Liu,
  • Yanlin Fu,
  • Haotian Jiang,
  • Hao Wu,
  • Yue Liu,
  • Xiaoxiao Lu,
  • Xiaohu Zhou,
  • Hongwei Li,
  • Rex T. Skodje,
  • Xingan Wang,
  • Bina Fu,
  • Wenrui Dong,
  • Dong H. Zhang,
  • Xueming Yang

摘要

Criegee intermediates are highly reactive species that play a pivotal role in the chemistry of the atmosphere, substantially impacting global climate and air quality. They are formed through the reaction of ozone with alkenes and considerably influence the formation of hydroxyl radicals and aerosols through their unimolecular decomposition and their reaction with key atmospheric components, respectively. However, their interaction with water vapour, a major atmospheric component, remains inadequately characterized. Here, using both time-dependent laser-induced fluorescence experiments and full-dimensional dynamics calculations, we investigate the reaction of syn-CH3CHOO, a prevalent Criegee intermediate, with water vapour. Our results reveal a much higher reaction rate than previously estimated, challenging the conventional notion that unimolecular decomposition dominates syn-CH3CHOO removal. Notably, we uncover a complex mechanism involving a roaming process that enhances reactivity. Our findings necessitate a revised assessment of reactions involving syn-mono- and di-substituted Criegee intermediates with water, which are crucial for accurately estimating the OH budget derived from these intermediates.